A new and simple multifunctional system based on hybrid calcite-poly(ethyleneimine) (PEI) nanostructured rods (NRs) formation, that shows as proof-of-concept sensing and removal (sensoremoval concept) of Pb2+ as a model toxic metal for environmental applications has been developed. The addition of Na2CaEDTA and CO32- solutions to a Pb2+ contaminated water guides to the crystallization of calcite-PEI NRs. These NRs are composed of self-assembly hexagonal plate-like shapes of around 450 nm. The just formed calcite-PEI NRs in suspension permit the Pb2+ detection, through a simple turbidimetric measurement, and at the same time act as Pb2+ remover. This sensing and removing system is able to detect up to 1 ppm Pb2+ (1-1000 ppm lineal range) and reaches an adsorption capacity of 240 mg Pb2+/g NRs as evaluated using 342 ppm of initial Pb2+ concentration at pH 4 after 30 min incubation time. This maximum Pb2+ removal capacity reported here is higher than other ones reported before using materials that are not as cheap and biodegradable as calcite. The Pb2+ detection range found for this system is suitable to evaluate levels of metal contamination from industrial wastewaters that use to be around 1-100 ppm. This system based on an advanced biodegradable material constitutes a useful tool as proof-of-concept in the design of future multifunctional platforms for the development of integrated environmental technologies with sensing and remediation functions.